Durability of Natural Fiber-reinforced

Composites of Ethylene–Propylene
Copolymer under Accelerated Weathering
and Composting Conditions

ANNAMALAI PRATHEEP KUMAR, DILIP DEPAN

AND RAJ PAL SINGH*
Division of Polymer Science and Engineering
National Chemical Laboratory
Dr. Homi Bhaba Road, Pune 411 008, India

ABSTRACT: Three types of composites are prepared by the melt mixing of

ethylene–propylene copolymer (EPC) with (i) 3% NaOH-treated jute fiber, (ii) 17.5%
NaOH-treated jute fiber, and (iii) commercial microcrystalline cellulose powder
using maleated EPC as compatibilizer. The composites obtained are characterized
by FTIR and microscopic measurements. Their mechanical properties are measured
using a UTM (Instron model 4204). The durability of the composites is evaluated in
an irradiation chamber with UV radiation of wavelength

290 nm and composting
conditions at different time intervals. The composites made from microcrystalline
cellulose show superior mechanical properties, biodisintegrability, as well as photo-
resistance whereas the specimen containing 3% NaOH-treated fiber exhibited
the lowest photoresistance. Increasing the quantity of maleated EP (MEP) in the
composition decreases photostability. Neat EPC has been found to be highly stable
than all the composites with increasing UV irradiation. It has been found that the
composites are less durable under both abiotic and biotic conditions in comparison
to the neat polymer.

KEY WORDS: composites, jute fiber, microcrystalline cellulose, mechanical

properties, compatibilization, photodegradation and composting.

*Author to whom correspondence should be addressed. E-mail: singh@poly.ncl.res.in

Journal of THERMOPLASTIC COMPOSITE MATERIALS, Vol. 18—November 2005 489

0892-7057/05/06 0489–20 $10.00/0 DOI: 10.1177/0892705705054411
ß 2005 Sage Publications
490 A. P. KUMAR ET AL.

INTRODUCTION

emerged as one of the alternatives

B IODEGRADABLE PLASTICS HAVE
to overcome the plastic waste disposal problem, which has arisen
due to the increased consumption of non-degradable polymers. The realiza-
tion that natural polymers can be developed as a viable alternative to
petroleum-based polymers has led to voluminous researches on additives
for polyolefins that can cause their degradation [1]. In recent years, the
consumption of fiber-reinforced composites has skyrocketed, not only
due to environmental concerns, but also for yielding a unique combination
of high performance, great versatility, and processing advantages at
favorable costs. They exhibit many advantages including low density, little
damage during processing and require little processing equipment, high
stiffness, and a relatively low price [2–4]. Among many other methods
used for improving compatibility, maleic anhydride–polypropylene (MAH–
PP) has been found to be very efficient in improving the filler dispersion
and compatibility in PP–cellulose composites [5–9]. Jute fiber has many
attractive properties like renewability, versatility, non-abrasiveness,
porosity, hydroscopicity, reactivity, viscoelasticity, combustibility, and bio-
degradability [10]. Table 1 shows the technical information on jute fiber
[11,12]. The mercerization of natural fibers is one of the cheapest and oldest
methods and its effectiveness has been found to depend on the concentration
of the alkaline solution, its temperature, time of treatment, tension of the
material as well as on the additives present [13,14]. According to Lai and
Sarkanen [15], the peeling process, which is degradation at the reducing ends
of cellulose chains, is relatively rapid at 150–190 C. Gentile et al. [16] had
also detected that the decrease in the concentration of the alkaline solu-
tion and the temperature reduced the peeling factor by the hydrolysis of
amorphous cellulose. On the other hand, it is well evident from the results
of theoretical calculations of fibers [17], that the quality of fibers in terms of

Table 1. Technical information on jute fiber [11–12].

Physical and mechanical properties

Density (g/cm3) Elongation (%) Tensile Young’s Moisture
modulus (MPa) modulus (MPa) absorption
1.3 1.5–1.8 393–773 26,500 12

Composition (%)

Cellulose Hemicellulose Pectin Lignin Water soluble

components
64.4 12.0 0.2 21–24 1.1
Durability of Natural Fiber-reinforced EPC Composites 491

mechanical properties depends on the degree of polymerization, crystal-

linity, orientation of chains (spiral angle), and fiber diameter. According to
Hermans [18] and Roy et al. [19,20], the alkali treatment will also affect the
fiber orientation by swelling, stretching, and reorientation. It will thus be
worthwhile to study the effect of the concentration of the alkaline solution
on the mechanical properties of fiber-reinforced composites.
Being multicomponent systems, the durability and performance of the
composite materials are of paramount importance. Therefore, the study
focuses on the durability of composites based on natural fibers in different
environmental conditions. Recently, Joseph et al. [21] have shown that the
effect of the chemical modifications of sisal fibers reduces the water uptake
and the UV susceptibility.
Only very few works are available in the literature on the biodegradation
of fiber-reinforced composites in different conditions, such as in an aqueous
media [22], terrestrial environment [23], and composting [24], where the
preparative methods affect the biodegradability of these composites. The
synthetic polyolefins based on ethylene–propylene copolymers (EPC) have
a wide range of applications from rigid thermoplastics to soft elastomers
by varying the ethylene–propylene monomer ratio. These polyolefins
were observed to be degraded by photooxidation [25,26], photoinduced
biodegradation [27], and in natural and accelerated composting conditions
[28]. The present study focuses on the effect of size and treatment of the jute
fibers on the mechanical properties and durability of their composites in
biotic and accelerated weathering conditions.

EXPERIMENTAL

Materials

The EPC (ethylene – 15.1 mol%, MFI – 3.5 g/10 min, and density
0.9 g/cm3) was obtained from M/s. Montell Ferrara, Italy. Maleic
anhydride, benzoyl peroxide, sodium hydroxide, and xylene were obtained
from M/s. SD Fine Chemicals Ltd., India. The jute fibers were purchased
from the local market and mercerized using an alkaline solution. The jute
fibers (EPC1) were treated with 3% NaOH aqueous solution for 3 h at
80–90 C. They were washed with deionized water upto the extent that the
pH of the resulting filtrate was 7.0 and dried in a vacuum oven at 50 C for
1 week. The same procedure was followed for the treatment of the second
batch of fibers using 17.5% of NaOH solution and the resulting composites
were named EPC2 and EPC4. The alkali-treated fibers were cut into short
pieces of 6 mm length. The microcrystalline cellulose (MC) powder, for the
492 A. P. KUMAR ET AL.

third fiber EPC3, for thin layer chromatography (TLC grade) was obtained
from M/s. Loba Chemie, Mumbai, India.

Preparation

MALEATION OF EPC
The dried EPC was maleated in a melt blender (Brabender plasticorder –
487106), with a chamber volume of 55 cm3, by melting in the presence of
benzoyl peroxide (0.15% wt/wt) and MAH (3% wt/wt) at 170 C at 65 rpm
for 1.5–2 min. Five grams of crude maleated EP (MEP) was dissolved
in 250 mL of xylene at 125 C for 3–5 h and then added to 750 mL of cold
acetone. The precipitated MEP was washed with acetone, filtered, and dried
in a vacuum oven at 50 C for 12 h.

PREPARATION OF COMPOSITES
The composites were prepared at 170 C with 70 rpm for 3 min as depicted
in Table 2. The samples were molded to obtain films (thickness 100 mm)
in an electrically preheated hydraulic Carver press at 180 C for 1.5 min and
quench cooled to room temperature (27 C).

Characterization

FTIR SPECTROSCOPY
The functional group analysis was done using a Perkin–Elmer 16 PC
FTIR spectrophotometer and we focused on the changes in the hydroxyl
(3600–3100 cm1) and carbonyl regions (1800–1600 cm1) that follows the
photooxidation.

Table 2. Composition of composites prepared.

Sample no. Description Code

1 Neat EP copolymer NeatEP
2 Maleated EP copolymer MEP
3 45 wt% EP copolymer þ 45 wt% maleated copolymer þ 10 wt% EPC1
of 3% NaOH-treated jute fiber
4 45 wt% EP copolymer þ 45 wt% maleated copolymer þ 10 wt% EPC2
of 17.5% NaOH-treated jute fiber
5 45 wt% EP copolymer þ 45 wt% maleated copolymer þ 10 wt% EPC3
of commercial microcrystalline cellulose powder
6 70 wt% EP copolymer þ 20 wt% maleated copolymer þ 10 wt% EPC4
of 17.5% NaOH-treated jute fiber
Durability of Natural Fiber-reinforced EPC Composites 493

MEASUREMENT OF MECHANICAL PROPERTIES

For tensile property estimations, the specimens were cut according to IS:
2508-1984 : A4. The static tensile behavior of composites was investigated
at room temperature (27  2 C) and 65  5% relative humidity using a
Universal Testing Machine (Instron model 4204) at a crosshead speed of
10 mm/min. The average value out of six measurements was reported for
each composition.

MICROSCOPIC MEASUREMENTS
The dimensions of fibers were determined using an optical microscope
(Olympus, Model B  50 F4, Japan) with 50 times magnification. The
surface morphological changes of photoirradiated and composted samples
were examined by staining the samples with osmium tetroxide, drying under
vacuum at 50 C for 24 h, and scanning under an electron microscope (Leica
Cambridge Stereoscan 440 Model).

Performance Evaluation

PHOTODEGRADATION
The samples were irradiated (
290 nm) in a polychromatic irradiation
chamber SEPAP12/24 (M/s Material Physico Chimique, Neuilly, Marne,
France) at 60 C under air. This polychromatic irradiation chamber consists
of (4  400 W) medium-pressure mercury vapor lamps supplying radiations
longer than 290 nm [24–28]. The changes in functional groups during photo-
oxidation were studied by FTIR spectroscopy. The changes in mechanical
properties were also determined by irradiating the tensile samples and
drawing as mentioned using a Instron 4204 (UTM).

BIODEGRADATION: COMPOSTING METHOD

The compostability tests were performed in a laboratory scale compost
bin, and the size of films was 4  4 cm2. The constitution of the solid waste
mixture (compost) used for biodegradability testing was as follows (dry
weight): 40.8% shredded leaves, 11.4% cow manure/dung, 15.8% news-
paper and computer paper, 2% white bread, 7.8% sawdust, 19.2% food
waste (dry milk, potato, carrot, banana, and other vegetables), and 3.0%
urea. The compost bin was covered with green grass and the moisture
content was maintained by spraying water periodically. To avoid anaerobic
conditions, the bin was constantly aerated with oxygen through a hollow
tube. The films were removed from the compost and washed thoroughly
with deionized water, dried in a vacuum oven at 50 C, up to a constant
weight. Again the samples were incubated in the compost. This process of
removal, washing, drying, and weighing was done every month for a period
494 A. P. KUMAR ET AL.

of six months. The gravitational weight losses of the films were measured
using a digital balance, Prescisa 205 A SCS, Switzerland. The compost-
ability was measured in terms of weight loss (%), using the formula:

Weight loss ð%Þ

¼ ½ðInitial weight ðgÞ  Final weight ðgÞÞ=Initial weight ðgÞ  100

RESULTS AND DISCUSSION

Figure 1 shows the optical micrographs of alkali-treated jute fibers

and microcrystalline cellulose powder. Their dimensions are presented
in Table 3. The chemical composition of the fibers with respect to their
cellulose and lignin content was determined by 1H-NMR spectroscopy,
measuring the areas of aromatic and aliphatic proton peaks [29,30].
Microcrystalline cellulose fibers were relatively smaller than other fibers.

Microcrystalline 3% NaOH 20 m 17.5% NaOH

20 m treated jute treated jute
cellulose

(a) (b)
Figure 1. Optical micrographs of fibers (a) microcrystalline cellulose and (b) jute fibers
(50 magnification).

Table 3. Characteristics of treated fibers.

3% NaOH- 17.5% NaOH- Microcrystalline

Parameters treated jute treated jute cellulose
Yield (%) in alkali 70.01 58.05 –
treatment
Length (mm) 6000  50 6000  50 38.8  0.2
Diameter (mm) 70.4  0.2 47.2  0.2 14.8  0.2
Aspect ratio (l/d) 85.22  0.5 127.11  0.5 2.62  0.2
Lignin content Higher Moderate Nil/low
Durability of Natural Fiber-reinforced EPC Composites 495

6
Absorbance

5
EPC4
4
EPC3
3 EPC2

2 EPC1

1 MEP
NeatEP
0
4000 3500 3000 2500 2000 1500 1000 500
-1
Wavenumber (cm )
Figure 2. FTIR spectra of composites.

Figure 2 shows the IR spectra of the neat polymer and composites prepared,
where the rising peaks at 1780 and 1713 cm1 can be attributed to the cyclic
anhydride and carboxylic acid groups.

Effect of Fiber Treatment

After the melt mixing of fibers with neat EP/MEP, the absorption peak
at 1780 cm1 decreased whereas at 1740–1720 cm1 it increased, which can
be attributed to ester formation. The possible interactions of fiber, com-
patibilizer, and polymer are schematically represented in Figure 3. The
interactions (a) and (b) are predominantly favored by solution impregna-
tion method while by extrusion method, complete esterification cannot
be expected [5,24]. Thus, in the composites prepared, the polar–polar
interactions (c) may be present. The ester formation, which is evidence of
compatibility [5] depends on the availability of hydroxyl groups on the
surface of the fibers. The area under the peak at the carbonyl region before
irradiation is shown, in Figures 2 and 6(a), to be higher for EPC3, indicating
more ester formation than in other fibers. This may be due to the higher
availability of hydroxyl groups on the surface, better dispersion, and higher
surface area of microcrystalline cellulose. The absorbance at the hydroxyl
region for EPC3 was observed to be higher than that for other composites.
This variation in hydroxyl and carbonyl groups may be attributed to the
496 A. P. KUMAR ET AL.

Polymer
Nonpolar
(hydrophobic)
matrix Nonpolar end Polar end
OC CO
O
OH OH
HO O
O O O
O HO
OH
OH

Polar (hydrophilic) fiber

OC CO OC CO
OC CO
O O O OH OH O

HO OH HO OH HO OH
OH OH OH

(a) (b) (c)

Figure 3. Schematic representation of interactions of compatibilizer on fiber.

extent of alkali treatments. The jute fiber was only alkali treated with
different concentrations whereas the commercial microcrystalline cellulose
was generally derived from multistage processes like water retting, alkali
mercerization, bleaching, and milling processes. On treatment with alkali,
the lignin which make the fibers stiffer and stronger by acting as an adhesive
between cellulose microfibrils by forming covalent hydrogen bonds, was
removed to a significant extent depending on the concentration used. With
lower concentrations of alkali (3%), lignin could be removed to a lesser
extent. The absorption bands at 1700–1630 cm1, especially at 1659 and
1639 cm1, were observed for the acidic and aldehydic carbonyl stretching of
lignin and other extractives [31] in the IR spectra of EPC1, EPC2, and EPC4
and they were hardly detectable in EPC3. The optical micrographs of EPC1,
EPC2, and EPC3 are shown in Figure 4, where it can be observed that after
processing, the fibers were destroyed and dispersed. It was observed that the
accumulation/population of the fibers in the middle of the film that was
pressed under the Carver press was higher in the case of EPC1 and EPC2
whereas in EPC3, the microfibers could be found even at the edges of
the film. Because of its smaller size, microcrystalline cellulose favors better
dispersion.
Durability of Natural Fiber-reinforced EPC Composites 497

20 µm

(a)

20 µm

(b)

20 µm

(c)
Figure 4. Optical micrographs of composites (a) EPC1, (b) EPC2, and (c) EPC3
(50 magnification).
498 A. P. KUMAR ET AL.

ON MECHANICAL PROPERTIES
By comparing the mechanical properties of EPC1, EPC2, and EPC3,
the effect of treatment on the fibers could be revealed. Figure 5 shows the
mechanical properties of all the composites. The modulus, which indicates
the stiffness of the materials, was found to be much improved in the case of
composites than that of the neat polymers. The order of increasing modulus
was observed for composites, as EPC1 > EPC3 > EPC2. With a constant
polymer–compatibilizer ratio, the difference in modulus of the composites
(EPC1 and EPC2) based on jute fibers could be attributed to the treatments
on the fibers. The content of lignin and other extractives might be higher
in the fibers used for EPC1 than that for EPC2 and EPC3. The presence
of lignin which acts as an adhesive between the cellulose chains, imparts
stiffness and strength to the fibers. The fibers used for EPC2, have been
treated by higher concentrations of the alkaline solution, which may
reduce the lignin content in the fibers. Thus, these composites have shown
a lower modulus. EPC3, based on microcrystalline powder has also
shown higher modulus. This could be attributed to the better dispersion

30

1400
27
Tensile modulus [MPa]

1200 24
Yield stress [MPa]

21
1000

18

800
15

600 12

NeatEP MEP EPC1 EPC2 EPC3 EPC4 NeatEP MEP EPC1 EPC2 EPC3 EPC4
30 90

80
27
70
Elongation at break [%]
Stress at break [MPa]

24 60

50
21
40
18
30

15 20

10
12
0

NeatEP MEP EPC1 EPC2 EPC3 EPC4 NeatEP MEP EPC1 EPC2 EPC3 EPC4

Figure 5. Mechanical properties of composites.

Durability of Natural Fiber-reinforced EPC Composites 499

of microcrystalline fibers throughout the matrix. The yield stress indicating

the hardness of the materials was observed to be higher in the composites
than that in the neat polymer. EPC3 was observed to be higher among
the composites while EPC2 was lower in yield strength. The efficiency of
stress transfer would be higher in EPC3 due to the better dispersion
of microcrystalline fibers. The stress at break that denotes the ultimate
strength of the material was also observed to be improved in the composites.
In this parameter also, EPC3 preceded others. The elongation at break (%),
which is related to the ductility of a material was observed to drop in
the case of composites. Among the composites, the elongation at break (%)
was lower for EPC1 whereas EPC3 showed a higher elongation. In the
composites, the entanglement and slippage of macromolecular chains, which
may happen during the tensile test were reduced due to the transfer of
applied stress to the fibers. The stress transfer to fibers, which can reduce the
deformation of the matrix mostly depends on the interfacial interactions.
The interfacial interactions were expected to be more in EPC3 because
of their better dispersion. In EPC1 and EPC2, the lack of better dispersion
will create more ‘incompatible centers’. These centers can act as ‘stress
concentrators’ where failure mechanism initiated by causing the local stress
in their vicinity to exceed the strength of the samples break at the initial
stages of the tensile tests. This may be the cause of lower values of
elongation (%) at break and yield strength of EPC1 and EPC2 than that of
EPC3.

ON DURABILITY/DEGRADABILITY
Photoirradiation
The photodegradation of polyolefins has been extensively studied. IR
spectroscopy is a conventional tool to examine photooxidation by
monitoring the rising peaks in the carbonyl and hydroxyl regions. Though
carbonyl and hydroxyl groups were already present in the composites, the
increase in these regions can be relatively observed during photoirradiation.
The increase in absorbance in the hydroxyl region is shown in Figure 6(a)
in terms of area under the peak. Figure 6(b) shows the increase in
absorbance in the carbonyl region with a maximum at 1720 cm1. The
decrease at 1780 cm1 for the cyclic anhydride group was observed after 25 h
of irradiation. The presence of the carbonyl group of MEP and the hetero-
aliphatic ring structure of the cellulose fiber was believed to accelerate the
photooxidation of all composites. The rate of increase in the absorbance was
found to be higher in the case of EPC1. This may be due to the presence of
photosensitive components i.e., aromatic based lignin components in the
jute fiber [32]. Among the composites, EPC3 was relatively less susceptible
to photooxidation. The crack formation on the surface of EPC1 and EPC3
500 A. P. KUMAR ET AL.

(a) -1
Hydroxyl region (3600-3100 cm )
180

160

140
Area under the peak 0h
120 50h
100h
100 150h

80

60

40

20

0
NeatEP MEP EPC1 EPC2 EPC3 EPC4
Samples

(b) -1
Carbonyl region (1800-1600 cm )
65
60
55
50
0h
Area under the peak

45
50h
40 100h
35 150h
30
25
20
15
10
5
0
NeatEP MEP EPC1 EPC2 EPC3 EPC4
Samples
Figure 6. (a) Changes in FTIR spectra at the hydroxyl region. (b) Changes in FTIR spectra at
the carbonyl region.

is shown in Figure 7(a) and (b). It is obvious that the crack formation
(amorphous) on the surface considerably accelerates the rate of auto-
photooxidation [33] further, as degradation is initiated from the amorphous
surface of the polymers.
Durability of Natural Fiber-reinforced EPC Composites 501

(a)

(b)
Figure 7. (a) Scanning electron micrograph (SEM) of 50 h of photoirradiated EPC1.
(b) Scanning electron micrograph (SEM) of 50 h of photoirradiated EPC3 (2 K
magnification).

The detrimental effect of photoirradiation on the mechanical properties

is shown in Figures 8–10. The moduli of the composites were found to
be increased at the beginning of irradiation. This may be attributed to
the cross-linking between polymeric chains. After 150 h of irradiation,
specimens of EPC1 became very brittle and therefore could not be handled
502 A. P. KUMAR ET AL.

2000

1800 NeatEP
MEP
Tensile modulus [MPa]

EPC1
1600
EPC2
EPC3
1400 EPC4

1200

1000

800

0 50 100 150
Irradiation time [h]
Figure 8. Changes in tensile modulus during photoirradiation.

80

NeatEP
70
MEP
12 EPC1
Elongation at break [%]

60

EPC2 50

EPC3 40
10
EPC4 30
Elongation at break [%]

20

10
8 0
0 50 100 150
Irradiation time [h]

0
-20 0 20 40 60 80 100 120 140 160
Irradiation time [h]
Figure 9. Changes in elongation at break (%) on photoirradiation.
Durability of Natural Fiber-reinforced EPC Composites 503
30 30
NeatEP
27 MEP
NeatEP
EPC1
24 25 MEP
EPC2
EPC1

Stress at break [MPa]

21 EPC3
EPC2
Yield stress [MPa]

EPC4
EPC3
18 20 EPC4
15

12 15

6 10

0 5
0 50 100 150 0 50 100 150

Irradiation time [h] Irradiation time [h]

(a) (b)

Figure 10. Changes in (a) yield stress and (b) stress at break during photoirradiation.

8
NeatEP
7 MEP
EPC1
6 EPC2
Weight loss [%]

EPC3
5 EPC4
4

0 1 2 3 4 5 6
Composting time [months]
Figure 11. Weight loss (%) of nonirradiated composites in composting.

for mechanical property measurements. The rate of brittleness formation

among the composites was in the order of EPC1
EPC2  EPC4 > EPC3.
Other material properties like yield stress, stress at break, and elongation
dramatically decreased with increasing time of irradiation.

On Biodegradation: Composting
Figure 11 shows the biodisintegrability of the nonirradiated samples in
terms of percentage weight loss under composting conditions. Neat EP
was observed to be the most stable in biodegradation. MEP was found to be
504 A. P. KUMAR ET AL.

disintegrated in the composting environment due to the functionality of its

polymer chain. The composites were more susceptible to microbial attack.
The hydrophilic nature and bioassimilability of fibers facilitate the microbial
adhesion on the surface of the composite films. In the initial days of
composting, weight loss was observed to be low for all the samples and it
increased with an increase in composting time. This can be attributed to the
fact that during the initial days of composting, the microorganisms may take
time to penetrate into the polymer matrix. In comparison, EPC3 showed
a higher weight loss than the alkali-treated fibers (in EPC1, EPC2, and
EPC4), which can be attributed to the treatment of the fibers. In the case of
composites, in which one component degrades faster than the other, the
weight loss in composting conditions is mostly due to the degradation of
that component. The polymer matrix would remain intact and the loss of
fibers from the composites may reduce the mechanical integrity of the
samples. Therefore, the nonirradiated composites cannot be true biode-
gradable materials, but they can be disintegrated. This disintegration might
facilitate the invasion of the microorganism, but not complete degradation
of the polymer matrix. The difference in weight loss (%) could be attributed
to the difference in bioaccessibility of the fibers only. In natural fibers (of
EPC1, EPC2, and EPC4), cellulose which is most susceptible to biotic
degradation is cross-linked (mostly phenolic linkage) with lignin and other
extractives. Since lignin is an aromatic based component, it could reduce the
bioaccessibility to the cellulose chains [34]. Thus, the composite based on
3% NaOH-treated fibers was relatively more stable than other composites
in composting conditions. Earlier studies had reported that [24,27] the
photoirradiated samples were more susceptible to bioassimilation due to the
formation of holes and cracks on the surface of the films. These amorphous
surfaces facilitate the adhesion and penetration of microorganisms into the
matrix. The crack formation on the composites during the photoirradiation
can also be observed in Figure 7(a) and (b) (SEMs of irradiated samples)
and it is apparent that photoinduced biodegradation of these composites
can be expected to be higher than that of nonirradiated samples. The
inherent and complete biodegradation of the polyolefin matrix (in the
composites also) requires pretreatment (photooxidation/thermooxidation).
Therefore, it is convenient to choose the pathways for disposal of the
commodities based on these natural fiber-reinforced composites of
polyolefins.

Effect of Compatibilization

It is evident from Figures 2 and 6(b) (oh)-before irradiation, that the ester
formation was comparatively higher in EPC2 than EPC4 and it is because of
Durability of Natural Fiber-reinforced EPC Composites 505

the higher amounts of MEP in EPC2 than in EPC4. So the chemical

compatibility between the polymer and fillers was favored by increasing the
amount of compatibilizer. The comparison of the properties of EPC2 and
EPC4 could depict the effect of compatibilization.

ON MECHANICAL PROPERTIES
The compatibilization of composites was in favor of increasing
mechanical properties. In Figure 5, it can be seen that the tensile
modulus of EPC4 was observed to be relatively higher than that of EPC2.
This can be attributed to the quantity of compatibilizer, which favors the
encapsulation of the fibers. The wetting of the fiber by increased amounts
of compatibilizer could give strong interfacial adhesion. The improved
compatibilization decreases the critical aspect ratio, so that the fibers
with a lower aspect ratio also become sufficiently long to bear the applied
stress [35]. The efficiency of the stress transfer in the composites is
largely determined by the interfacial structure. Thus we can expect that the
efficiency of the transfer of applied stress in EPC2 is higher than that
in EPC4. The difference in modulus may be attributed to the fact that
during the tensile test, the strain/deformation was observed to be higher
for EPC2 for the same applied stress than that for EPC4, because the
entanglement and mobility of macromolecular chains were favored in
EPC2 [36]. Then, the yield stress, which denotes the hardness of the
materials, was observed to be higher for EPC4 than for EPC2. It can be
expected that the higher compatibilizer amount would increase the yield
stress value because of more compatibilization and higher stress transfer.
Contrarily, EPC4 shows a higher value. This may be attributed to the fact
that at the yield point, EPC2 undergoes more strain than EPC4 at the yield
point and ultimately results in a lower yield stress value for EPC2. The
effect of compatibilization could also be observed as the elongation (%) at
break of EPC2 and EPC4 were 6.9 and 5.8, respectively. The
reduced amount of compatibilizer in EPC4 would improve the modulus
and hardness of the composite material. In other words, the compatibiliza-
tion by increasing the amount of the compatibilizer would improve the
ultimate strength and elongation at break (%), which is directly related to
the toughness of the material. However, the difference in these properties
was no more significant in the case of reinforcing the materials.
As found by Kazayawoko et al. [31], the chemical compatibility like
ester bond formation is not a key determinant factor for improving the
mechanical properties. The other factors are for improving the mechanical
properties, reduction in surface energy, polarity, and mechanical inter-
locking [31,37].
506 A. P. KUMAR ET AL.

ON DURABILITY
Photoirradiation
In Figure 6(a) and (b), the increase in absorbance at the hydroxyl and
carbonyl regions is found to be higher in EPC2 than that in EPC4. As the
amount of compatibilizer was higher in EPC2 than in EPC4, the carbonyl
groups, such as anhydride, lactone, ester, aldehyde, and ketone would be
more in EPC2. The presence of carbonyl groups and heteroatom in the
polymer sensitizes the photodegradation via hydrogen abstraction from
polymer chains. Thus, the chemical compatibilization between the polymer
and the fiber was observed to increase photooxidation.

Biodegradation
Figure 11 shows the percentage weight loss of nonirradiated composites.
During the initial days of composting, both EPC2 and EPC4 showed almost
the same low rate of weight loss. In this period, microorganisms might
penetrate into the matrix. The ester group, which had more of a presence in
EPC2 than in EPC4, favors the microbial adhesion. After 3 months of
composting, the percentage weight loss of EPC2 was found to be higher
than in EPC4, as has been observed by earlier studies [24,38]. The
photoirradiation imparts more degraded products (low molecular weight
and functional group containing compounds) in composites, so the
photoinduced biodegradation will be higher in the case of more
compatibilized composites. So, the compatibilization was found to increase
the degradability of the composite materials.

CONCLUSIONS

The mechanical, physical, and thermal properties and the durability of the
natural fiber-reinforced composites depend on their chemical constituents
and preparation methods. The different treatments on the fiber affect the
quality of fiber and ultimately the properties of the composites. From our
investigation, the mechanical properties of the composites were observed to
be better than that of neat polymers. The variation in mechanical properties
of all the composites was attributed to the treatment on the fibers. Under
UV irradiation and composting environment, the neat polymer matrix
exhibited higher resistance to photooxidation and biodisintegration than
the composites. Among the composites, EPC1 was more susceptible to
photooxidation than others while the composite based on commercial
microcrystalline cellulose was more stable. EPC1 prepared with jute fiber
treated with an alkaline solution of low concentration, exhibited lower
biodisintegrability. As higher concentrations of the alkaline solution
reduce the content of lignin and other extractives and the bioaccessibility
Durability of Natural Fiber-reinforced EPC Composites 507

of the fiber becomes easier, EPC2 and EPC4 are more susceptible to
biodisintegration in comparison to EPC1. The composites based on
commercial cellulose showed relatively higher photostability and also
biodisintegrability among the composites. We conclude that the durability
and mechanical properties of the natural fiber-reinforced composites can be
optimized by selecting the appropriate treatment for the fibers.

ACKNOWLEDGMENT

The authors are grateful to Dr S. Sivaram, Director, National Chemical

Laboratory, for his fruitful discussions and encouragement.

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